EP1923934A1 - pile électrochimique rechargeable - Google Patents

pile électrochimique rechargeable Download PDF

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Publication number
EP1923934A1
EP1923934A1 EP06023611A EP06023611A EP1923934A1 EP 1923934 A1 EP1923934 A1 EP 1923934A1 EP 06023611 A EP06023611 A EP 06023611A EP 06023611 A EP06023611 A EP 06023611A EP 1923934 A1 EP1923934 A1 EP 1923934A1
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EP
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Prior art keywords
positive electrode
battery cell
cell according
active
porous structure
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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EP06023611A
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German (de)
English (en)
Inventor
Günther Hambitzer
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
FORTU INTELLECTUAL PROPERTY AG
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FORTU INTELLECTUAL PROPERTY AG
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Publication date
Application filed by FORTU INTELLECTUAL PROPERTY AG filed Critical FORTU INTELLECTUAL PROPERTY AG
Priority to EP06023611A priority Critical patent/EP1923934A1/fr
Priority to ES07819736.5T priority patent/ES2574564T3/es
Priority to AU2007321466A priority patent/AU2007321466B2/en
Priority to MX2009003977A priority patent/MX2009003977A/es
Priority to PCT/EP2007/009744 priority patent/WO2008058685A1/fr
Priority to KR1020097012224A priority patent/KR101639238B1/ko
Priority to US12/513,547 priority patent/US8906556B2/en
Priority to CN2007800421831A priority patent/CN101622738B/zh
Priority to BRPI0718646A priority patent/BRPI0718646B1/pt
Priority to EP07819736.5A priority patent/EP2089924B1/fr
Priority to CA2669551A priority patent/CA2669551C/fr
Priority to RU2009117719/07A priority patent/RU2438212C2/ru
Priority to JP2009535631A priority patent/JP5356240B2/ja
Publication of EP1923934A1 publication Critical patent/EP1923934A1/fr
Priority to IL198445A priority patent/IL198445A/en
Priority to ZA200904054A priority patent/ZA200904054B/xx
Priority to HK10106403.6A priority patent/HK1140313A1/xx
Withdrawn legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/80—Porous plates, e.g. sintered carriers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0568—Liquid materials characterised by the solutes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0569—Liquid materials characterised by the solvents
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/40—Alloys based on alkali metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
    • H01M6/162—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the invention relates to a, preferably non-aqueous, rechargeable electrochemical battery cell having a negative electrode, an electrolyte and a positive electrode, and a memory for storing active metal, which results in charging the cell from the electrode reaction at the negative electrode.
  • the invention is particularly directed to a battery cell in which the active metal (whose oxidation state is changed upon charge and discharge of the cell due to the electrode reaction occurring at the negative electrode) is an alkali metal, alkaline earth metal or a metal of the second subgroup of the Periodic Table, wherein lithium is particularly preferred.
  • the active metal whose oxidation state is changed upon charge and discharge of the cell due to the electrode reaction occurring at the negative electrode
  • the active metal is an alkali metal, alkaline earth metal or a metal of the second subgroup of the Periodic Table, wherein lithium is particularly preferred.
  • lithium will be referred to as the negative electrode active metal without loss of generality.
  • the electrolyte used in the invention is preferably based on SO 2 .
  • SO 2 electrolytes "in SO 2 based electrolyte” are referred to the electrolyte containing SO 2 not only as an additive in low concentration, but which causes the mobility of the ions of the supporting electrolyte contained in the electrolyte and the charge transport , at least partially ensured by the SO 2 .
  • the conductive salt is preferably a tetrahaloaluminate of the alkali metal, for example LiAlCl 4 , used.
  • a rechargeable alkali metal cell having an SO 2 -based electrolyte is referred to as a rechargeable alkali metal SO 2 cell.
  • the invention also relates to cells with other electrolytes which contain other conducting salts (e.g., halides, oxalates, borates, phosphates, arsenates, gallates) and other solvents which ensure the mobility of the ions.
  • these may be inorganic solvents (for example, sulfuryl chloride, thionyl chloride), organic solvents (for example, ethers, ketones, carbonates, esters) and ionic liquids. It is also possible to use mixtures of said other conductive salts and solvents with one another and with the abovementioned preferred conductive salts and solvents.
  • the required safety is an important issue. In many cell types in particular a strong warming can lead to safety-critical conditions. It may happen that the cell case bursts or at least leaks and harmful gaseous or solid substances escape or even fire.
  • thermo runaway a strong increase in temperature in the cell interior leads to the fact that exothermic reactions take place to a greater extent, which in turn lead to a further increase in temperature. This self-reinforcing effect is called "thermal runaway”.
  • Battery manufacturers attempt to control the charging or discharging circuit by electronic, mechanical or chemical mechanisms so that the flow of current is interrupted below a critical temperature so that no "thermal runaway” can occur.
  • electronic, mechanical or chemical mechanisms so that the flow of current is interrupted below a critical temperature so that no "thermal runaway” can occur.
  • pressure-sensitive mechanical or temperature-sensitive electronic switches are integrated.
  • alkali metal battery cells particularly Li-ion cells
  • the lithium which results from charging the cell from the electrode reaction at the negative electrode (by incorporation of an electron), is embedded in the layer lattice of the graphite in the case of Li-ion cells. Lithium-ion cells therefore do not contain any accumulations of metallic lithium in normal operation.
  • alkali metal cells are of great practical importance, especially because they are characterized by a high cell voltage and a high energy density (electrical capacity per unit volume) and high specific energy (electrical capacity per unit weight).
  • the invention is based on the problem of further improving battery cells, in particular alkali metal cells, with regard to performance data (energy density, power density) while at the same time having very good safety properties.
  • a rechargeable battery cell of the type explained in the introduction in which the cell contains a porous structure in which the active material of the positive electrode is contained and disposed in the vicinity of an electronically conductive substrate of the negative electrode such that at least a portion of the active metal resulting from the electrode reaction at the negative electrode penetrates and is stored in the pores of the porous structure containing the positive electrode active material wherein the storage of the active metal in the pores of the porous structure containing the positive electrode active material occurs, at least in part, by deposition in metallic form.
  • the active material of the positive electrode is a component of the cell which changes its charge state during the redox reaction taking place at the positive electrode.
  • the active material of the positive electrode is preferably an intercalation compound into which the active metal can be incorporated.
  • metal compounds are suitable (for example, oxides, halides, phosphates, sulfides, chalcogenides, selenides), in particular compounds of a transition metal M, in particular an element of atomic numbers 22 to 28 including mixed oxides and other mixed compounds of the metals are suitable. Lithium cobalt oxide is particularly preferred. When discharging such a cell, ions of the active metal are incorporated into the positive active mass.
  • the required separation of the active materials is usually achieved by being contained in spatially separated layers, which are usually separated by a separator.
  • a separator is referred to in battery technology, a material that is suitable to isolate the electrodes, in particular their active masses from each other in terms of electronic conduction, but on the other hand to allow the required ionic conduction.
  • the separator separates the total volume of the battery cell into two partial spaces, namely a positive electrode space and a negative electrode space, between which a charge exchange by the ions of the conducting salt is possible, but an electronic charge exchange is impossible. This applies regardless of the cell shape, that is, for example, for winding cells, in which the subspaces are formed as thin parallel layers wound around a common axis.
  • Interpenetrating electrodes are recommended for battery cells. According to the document, these are electrodes that form a network that extends in two or three dimensions, with each electrode penetrating the other. In comparison to the usual thin-film cells, this should result in an increased power density (with an unchanged high energy density).
  • the interdigitated electrodes consist of insertion materials, preferably intercalation materials, in whose lattice structure the active metal is bound.
  • the invention relates to cells in which the active metal is at least partially deposited in metallic form (ie, not bound within an insertion or intercalation electrode) during the charging process.
  • metallic form ie, not bound within an insertion or intercalation electrode
  • the W02003 / 061036 proposed to provide, in direct contact with the electronically conductive substrate of the negative electrode, a layer having a microporous structure whose pore size is dimensioned so that the active material deposited during the charging process grows into its pores in a controlled manner, which is therefore also referred to as a "deposition layer" ,
  • the pores of the deposition layer are to be completely filled by the active material growing into the porous structure in such a way that they are in contact with the electrolyte essentially only over the relatively small boundary surfaces at which (within the pores) the further deposition takes place.
  • the publication describes additional measures with regard to the layer structure of the deposition layer, which ensures the desired pore size and porosity as well as the required safety as well as possible. This includes the use of multiple materials of different grain size to form the porous structure and the use of an additional salt incorporated into the deposition layer.
  • an electrode construction is not only possible but even particularly advantageous, in which the positive electrode active material and the negative electrode active metal deposited on charging the electrode are not in separate (usually layered) electrode spaces but the active metal grows at least partially in metallic form into a porous structure containing its active mass.
  • the active metal grows at least partially in metallic form into a porous structure containing its active mass.
  • the porous structure consists of a structure-forming material (solid) and the pores (preferably homogeneous) distributed therein.
  • any structure can be used whose porosity is suitable for accommodating the lithium deposited during charging of the cell.
  • a porous structure formed from particles wherein the structure-forming
  • particles are interconnected to form a contiguous particle composite structure.
  • the porous structure containing the active material of the positive electrode may also consist of particles not connected to one another, whereby it must be ensured by suitable measures (eg, by puncturing into the cell, pressing) that the particles are in such close and firm contact with one another stand that the required electronic conductivity is guaranteed.
  • the porous structure containing the positive electrode active material contains within its structure-forming material an electronically conductive material as a conductivity improver.
  • an electronically conductive material for example, carbon particles or metal particles (e.g., baubles, chips, etc.) are suitable. Carbon is particularly preferred.
  • the structure-forming particles can be introduced into a metal foam (for example nickel foam) to form the porous structure containing the positive active material. It is also possible 'to fix them by pressing or by means of a binder on a metal or expanded metal.
  • the porous structure containing the positive electrode active material preferably forms a layer extending in parallel with the electronically conductive negative electrode substrate (also referred to as a drain member hereinafter). It is also referred to below as "porous positive electrode layer".
  • the cell according to the invention preferably has only two layers, namely the generally very thin dissipation element (substrate) of the negative electrode and the relatively much thicker positive electrode layer. The required cell volume is thus determined essentially by the volume of the positive electrode layer. An additional capacity for the deposited during loading of the cell active metal is not required. As a result, a substantial increase in the energy density is achieved. According to the present investigations can be according to the invention reach a practical energy density of more than 1.5 kWh / l.
  • the reaction components are homogeneously mixed so that optimum reactivity is ensured. If the components are not homogeneously distributed but spatially separated, as in the electrode layers of a conventional battery, the actual explosive capacity is higher than expected according to the calculated BRP. From a value of BRP of 1200 x 10 6 kJ / m 3 one speaks of an explosive substance.
  • the system lithium / lithium cobalt oxide with inorganic electrolyte solution LiAlCl 4 xSO 2 has a value of about 200x10 6 kJ / m 3 .
  • a macroscopically homogeneous mixture can be assumed so that the calculated value of the BRP is a substantially correct measure of the actual explosion safety.
  • the invention leads to an "inherently safe" cell, ie to a battery cell whose safety is not based on additional external security measures, but on their physicochemical properties and internal design features. It is also important that only very little electrolyte is needed.
  • the volume of the electrolyte in the cell corresponds to at most twice, more preferably at most, the simple free pore volume of the porous structure of the positive electrode.
  • an additional salt in addition to the conductive salt, in addition to the conductive salt, an additional salt, in particular a halide, especially preferably a fluoride may be contained in the cell.
  • the cation of the salt additive can be identical to the cation of the conductive salt, but also different.
  • Preferred cation of the additional salt is Li + or another alkali metal cation.
  • the salt additive is preferably contained in the electrolyte.
  • the invention is particularly advantageous in connection with a battery cell according to the international patent application WO 00/79631 A1 to use, which can be operated with a very small amount of electrolyte. It is a cell whose negative electrode in the charged state contains an active metal, in particular an alkali metal, whose electrolyte is based on sulfur dioxide and which has a positive electrode containing the active metal and from the ions in the electrolyte during charging escape.
  • the electrolyte is based on sulfur dioxide.
  • a self-discharge reaction takes place in which the sulfur dioxide of the electrolyte reacts with the negative electrode active metal to a sparingly soluble compound.
  • the electrochemical charge amount of the sulfur dioxide contained in the cell is smaller than the charge amount of the active metal that can be stored electrochemically theoretically in the positive electrode.
  • the battery cell can be operated with a significantly reduced amount of electrolyte and yet improved function.
  • a binder is present in the porous structure to produce a particle composite, it should have a not too high volume fraction of less than 50%, preferably less than 30% of the total solids volume of the porous structure.
  • the binder content is so low that it sits only in the region of the contact points between the structure-forming particles. Therefore, binder contents (volume ratio of the binder to the total volume the patterning particle) of less than 20% or even less than 10% is particularly preferred.
  • the positive active material is preferably contained in the porous structure of the positive electrode layer in a proportion of at least 50% by weight.
  • the structure-forming particles of the porous structure predominantly, ie with a proportion of at least 80%, from the material of the positive active material.
  • a binder for example, polytetrafluoroethylene is suitable.
  • the porosity of the porous positive electrode layer i. the volume ratio between the pores and the total volume can vary considerably.
  • the porosity in the porous positive electrode layer is between 20 and 80%, preferably between 25 and 75%, and more preferably between 25 and 50%.
  • the total pore volume should only be insignificantly greater than the volume of the maximum active metal deposited on the substrate of the negative electrode during charging.
  • the mean diameter of the pores of the porous positive electrode layer should be in their order of magnitude. This usually corresponds to about 1 to 2 ⁇ m in an SO 2 based electrolyte. Smaller values can lead to an increase in the overvoltage required for charging, but are basically possible. Even larger average pore diameters may be acceptable depending on the application.
  • the mean pore diameter of the porous positive electrode layer should be at most 500 ⁇ m, preferably at most 100 ⁇ m, and particularly preferably at most 10 ⁇ m.
  • the intraporous separator layer is preferably generated at least in part within the cell (in situ). This happens especially during the loading of the cell.
  • the first generation of the intraporous separator layer can take place during first charging cycles of the battery cell.
  • the intraporous separator layer can also be formed or renewed during the further operation. This is especially true in case of damage to the layer. Missing parts of the intraporous separator layer are newly formed or supplemented during the subsequent charging cycles. This repair mechanism is maintained throughout the life of the cell and inherently ensures safe and functional cells.
  • a reaction mechanism by which a cover layer suitable as an intraporous separator layer is formed on the inner surface of the porous positive electrode layer is possible in various cell systems.
  • General rules for the selection of suitable cell systems can not be specified, but it is readily possible, with the knowledge of the present invention, to test potentially suitable cell systems for the desired formation of an intraporous separator layer in them (especially when loading the cell).
  • an electrolyte containing SO 2 is particularly suitable.
  • it does not necessarily have to be an SO 2 based electrolyte as defined above.
  • the SO 2 can also be used in a lower concentration in admixture with another electrolyte (examples have been mentioned above), and in particular also mixtures with electrolytes containing organic solvents are possible.
  • an intraporous separator layer in situ or coating during production prior to initial loading of the cell
  • a coating method may be performed in which the porous positive electrode layer is partly (preferably for the most part) coated before the first charging process by one of the methods described above, but the complete intraporous separator layer is formed only during the operation of the cell (ie in particular during the first charging cycles).
  • the housing 1 of the battery 2 shown in Figure 1 consists for example of stainless steel and includes a plurality of battery cells 3, each having a positive electrode 4 and a negative electrode 5.
  • the electrodes 4, 5 are connected to terminal contacts 8, 9 via electrode terminals 6, 7 as is customary in battery technology. They are - as usual - formed as layers with a small in relation to their surface area thickness.
  • a bipolar structure (series connection) is also possible.
  • a special feature of the electrode arrangement of cells according to the invention separately shown in FIG. 2 is that the electronically conductive substrate 12, which forms the negative electrode lead-off element, directly adjoins a porous structure 13 (porous positive electrode layer) containing the active material of the positive electrode, that lithium deposited during the charging of the cell (negative electrode active material) penetrates into its pores 14.
  • the drain electrode 12 of the negative electrode is much thinner than the porous positive electrode layer.
  • the schematic representations of the figures are not to scale.
  • the porous positive electrode layer is at least ten times as thick as the electronically conductive layer forming the diverting element 12.
  • the electrodes 4, 5 are not located in the cells according to the invention in separate layers (macroscopically separated subspaces of the cell), but the active mass of the positive electrode is at the same time a structural component of a porous layer, in the pores of which the lithium is taken up during charging of the cell and at least partially deposited in metallic form.
  • the usual spatial separation of the parts of the cell that provide the required uptake capacity for lithium and the parts of the cell containing the positive active mass in separate layers is not given.
  • the cell only contains the two functional layers shown in the figures, namely the electronically conductive substrate 12 of the negative electrode and the porous positive electrode layer 13.
  • Figure 2 shows a highly simplified schematic representation of a microscopic enlargement of a section of the porous positive electrode layer 13 in the vicinity of the negative diverter 12.
  • structure-forming particles 16 of the layer 13 which in the illustrated embodiment of the active material 17 of the positive electrode 4 (eg LiCoO 2 ) exist.
  • the structure-forming particles 16 are connected to each other by means of a binder 19, the amount of which is concentrated so that it is concentrated only where the structure-forming particles 16 adjacent to each other, but otherwise remain numerous communication channels between the pores 14 of the porous positive electrode layer 13.
  • the pores 14 of the layer 13 are filled with electrolyte 21 before the first charging process. Methods by which it can be ensured that the electrolyte also penetrates into fine pores of a porous layer during filling are known. A suitable method is for example in WO 2005/031908 described.
  • FIG. 2 shows how the active metal 24 of the negative electrode, for example lithium, grows into the pores 14 of the porous positive electrode layer 13 when it is deposited on the surface of the discharge element 12 when the cell is charged.
  • the required separation of the active masses 24,17 of the two electrodes is ensured by an intraporous separator layer 25, which covers the entire Inner surface of the porous positive electrode layer 13, so the surface of the structure-forming particles 16 covered.
  • the intraporous separator layer is formed in situ, this formation process taking place predominantly during the first charge cycles.
  • the formation of the intraporous separator layer can be done both by the manufacturer of the battery, as well as the user.
  • the porous positive electrode layer 13 is disposed so close to the substrate 12 of the negative electrode 5 that there are no voids therebetween in which accumulations of active metal 24 deposited upon charging of the cell may form in metallic form.
  • such cavities should preferably not be significantly larger than the pores of the porous positive electrode layer 13.
  • a material 23 storing the negative electrode active metal which is referred to below as a lithium-storing material without loss of generality.
  • a lithium-storing material are different solids, which have the property that they can absorb lithium in itself. These include, in particular, graphite, intercalation compounds and lithium alloying metals.
  • the electronically conductive substrate 12 may be formed entirely of metal, preferably nickel.
  • a simple nickel sheet is suitable, but other metal structures, in particular in the form of a perforated plate or the like, are also possible.
  • the electronically conductive substrate 12 of the negative electrode also consists at least partially of a material storing its active metal, in particular of a lithium-storing material.
  • a deposition of active metal in metallic form takes place in the pores of the layer 13.
  • FIG. 4 shows as a result of the voltammetric investigations with the described experimental arrangement with the electrolyte LiAlCl 4 .1.5 SO 2 and an addition of 3% LiF the cycle efficiency E z plotted over the cycle number N z for 70 cycles.
  • the Zykleneffizienz is defined as the percentage of discharged when unloading the cell electrical energy (discharge capacity) in relation to the electric power consumed for charging (charging capacity).
  • experimental electrodes were prepared with lithium cobalt oxide mixed with 1.5% by weight of Aerosil and 1.5% by weight of powdered borosilicate glass. The dry mixed substances were taken up in water. The thermal treatment was carried out at 500 ° C for 25 minutes. The examination of three-electrode cells prepared with these experimental electrodes analogous to Experiment 1 led to substantially identical results.
  • the glass in its initial state does not necessarily have to be ion-conducting. It has been found that an ion-conducting glass can also be formed in situ from a non-ionic glass, in particular borosilicate glass, this being attributed to a reaction sequence in which first of the lithium cobalt oxide of the positive electrode by reaction with water lithium hydroxide and then from the Lithium hydroxide is formed to absorb water lithium oxide, which is incorporated into the glass and causes the required ion conductivity.
  • a non-ionic glass in particular borosilicate glass
  • Figure 5 shows results of these experiments, in which the ratio of the cell capacity (C E ) to the rated capacity (C N ) in% and the internal resistance Ri of the cell are plotted after 1 mS and after 5 seconds against the number of the charging cycle , One recognizes a continuous increase of the capacity up to 100% of the nominal capacity within the first 20 cycles and a substantially constant course of the resistance values.
  • the intraporous separator layer in the case of the battery system under investigation is caused by reactions which are triggered by short-term very high local currents, which flow on the LiCoO 2 upon impact of lithium and trigger reactions of the electrolyte components or of secondary products Usually be formed in occurring in the cell reactions.
  • the electrolyte components are LiAlCl 4 and SO 2 .
  • Secondary products are formed, for example, during charging and overcharging, for example in the form of lithium chloride (LiCl), aluminum chloride (AlCl 3 ) or lithium dithionite (Li 2 S 2 O 4 ) or sulfuryl chloride (SO 2 Cl 2 ).
  • the invention is not limited to the system under investigation.
  • the construction according to the invention is not suitable for every battery system.
  • electrolyte based on SO 2 other electrolytes, including organic electrolytes, have the property of being able to form stable cover layers which have the necessary electronically insulating properties but have ionic conductive properties.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
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EP06023611A 2006-11-14 2006-11-14 pile électrochimique rechargeable Withdrawn EP1923934A1 (fr)

Priority Applications (16)

Application Number Priority Date Filing Date Title
EP06023611A EP1923934A1 (fr) 2006-11-14 2006-11-14 pile électrochimique rechargeable
CN2007800421831A CN101622738B (zh) 2006-11-14 2007-11-10 可再充电的电化学蓄电池组电池
CA2669551A CA2669551C (fr) 2006-11-14 2007-11-10 Element de batterie electrochimique rechargeable
MX2009003977A MX2009003977A (es) 2006-11-14 2007-11-10 Celda de bateria electroquimica recargable.
PCT/EP2007/009744 WO2008058685A1 (fr) 2006-11-14 2007-11-10 Élément de batterie électrochimique rechargeable
KR1020097012224A KR101639238B1 (ko) 2006-11-14 2007-11-10 재충전 가능한 전기화학 배터리 셀
US12/513,547 US8906556B2 (en) 2006-11-14 2007-11-10 Rechargeable electro chemical battery cell
ES07819736.5T ES2574564T3 (es) 2006-11-14 2007-11-10 Célula de batería electroquímica recargable
BRPI0718646A BRPI0718646B1 (pt) 2006-11-14 2007-11-10 célula de bateria eletroquímica recarregável
EP07819736.5A EP2089924B1 (fr) 2006-11-14 2007-11-10 Élément de batterie électrochimique rechargeable
AU2007321466A AU2007321466B2 (en) 2006-11-14 2007-11-10 Rechargeable electro chemical battery cell
RU2009117719/07A RU2438212C2 (ru) 2006-11-14 2007-11-10 Перезаряжаемый элемент аккумуляторной батареи
JP2009535631A JP5356240B2 (ja) 2006-11-14 2007-11-10 再充電可能な電気化学電池
IL198445A IL198445A (en) 2006-11-14 2009-04-28 Rechargeable electrochemical battery cell
ZA200904054A ZA200904054B (en) 2006-11-14 2009-06-10 Rechargeable electro chemical battery cell
HK10106403.6A HK1140313A1 (en) 2006-11-14 2010-06-30 Rechargeable electro chemical battery cell

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AU (1) AU2007321466B2 (fr)
BR (1) BRPI0718646B1 (fr)
CA (1) CA2669551C (fr)
ES (1) ES2574564T3 (fr)
HK (1) HK1140313A1 (fr)
IL (1) IL198445A (fr)
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WO2015067795A1 (fr) * 2013-11-11 2015-05-14 Professorenbüro G. Hambitzer Prof. Dr. Rer. Nat. Habil. Günther Hambitzer Élément au lithium, électrochimique et rechargeable, doté d'un électrolyte contenant du dioxyde de soufre
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JP5356240B2 (ja) 2013-12-04
BRPI0718646B1 (pt) 2018-12-11
ES2574564T3 (es) 2016-06-20
CN101622738A (zh) 2010-01-06
IL198445A0 (en) 2010-02-17
JP2010509719A (ja) 2010-03-25
BRPI0718646A2 (pt) 2013-11-19
WO2008058685A1 (fr) 2008-05-22
AU2007321466A1 (en) 2008-05-22
RU2438212C2 (ru) 2011-12-27
CN101622738B (zh) 2013-09-18
KR101639238B1 (ko) 2016-07-13
AU2007321466B2 (en) 2011-11-03
CA2669551A1 (fr) 2008-05-22
EP2089924A1 (fr) 2009-08-19
US20100062341A1 (en) 2010-03-11
EP2089924B1 (fr) 2016-04-13
KR20090088405A (ko) 2009-08-19
IL198445A (en) 2015-02-26
HK1140313A1 (en) 2010-10-08
CA2669551C (fr) 2016-01-12
MX2009003977A (es) 2009-06-23
RU2009117719A (ru) 2010-11-20
US8906556B2 (en) 2014-12-09
ZA200904054B (en) 2010-04-28

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